Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts

Mistry, Hemma; Choi, Yong‐Wook; Bagger, Alexander; Scholten, Fabian; Bonifacio, Cecile S.; Sinev, Ilya; Divins, Nuria J.; Zegkinoglou, Ioannis; Jeon, Hyo Sang; Kisslinger, Kim; Stach, Eric A.; Yang, Judith C.; Rossmeisl, Jan; Roldan Cuenya, Beatriz

doi:10.1002/anie.201704613

Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts

Journal Article · Thu Aug 10 00:00:00 EDT 2017 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201704613· OSTI ID:1433976

^[1]; Choi, Yong‐Wook ^[2]; Bagger, Alexander ^[3]; Scholten, Fabian ^[2]; Bonifacio, Cecile S. ^[4]; Sinev, Ilya ^[2]; Divins, Nuria J. ^[2]; Zegkinoglou, Ioannis ^[2]; Jeon, Hyo Sang ^[2]; Kisslinger, Kim ^[5]; Stach, Eric A. ^[5]; Yang, Judith C. ^[4]; Rossmeisl, Jan ^[6]; ^[7]

Ruhr Univ., Bochum (Germany). Dept. of Physics; Univ. of Central Florida, Orlando, FL (United States). Dept. of Physics
Ruhr Univ., Bochum (Germany). Dept. of Physics
Copenhagen Univ. (Denmark). Dept. of Chemistry
Univ. of Pittsburgh, PA (United States). Chemical and Petroleum Engineering and Physics
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
Univ. of Copenhagen (Denmark). Dept. of Chemistry
Ruhr Univ., Bochum (Germany). Dept. of Physics; Fritz-Haber Inst. of the Max Planck Society, Berlin (Germany). Dept. of Interface Science

Efficient, stable catalysts with high selectivity for a single product are essential if electroreduction of CO₂ is to become a viable route to the synthesis of industrial feedstocks and fuels. A plasma oxidation pre-treatment of silver foil enhances the number of low-coordinated catalytically active sites, which dramatically lowers the overpotential and increases the activity of CO₂ electroreduction to CO. At -0.6 V versus RHE more than 90 % Faradaic efficiency towards CO was achieved on a pre-oxidized silver foil. While transmission electron microscopy (TEM) and operando X-ray absorption spectroscopy showed that oxygen species can survive in the bulk of the catalyst during the reaction, quasi in situ X-ray photoelectron spectroscopy showed that the surface is metallic under reaction conditions. Finally, DFT calculations reveal that the defect-rich surface of the plasma-oxidized silver foils in the presence of local electric fields drastically decrease the overpotential of CO₂ electroreduction.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-06CH11357; FG02-03ER15476; SC0012704

OSTI ID:: 1433976

Alternate ID(s):: OSTI ID: 1374678

Report Number(s):: BNL-203511-2018-JAAM

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 38 Vol. 56; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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